JP9401176 '-'AER 1-M JAERI-M 93-222...JAERI-H—93-222 JP9401176 JAERI-M 93-222 h»; TWcomm® 1 9 9...
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JAERI-H—93-222 JP9401176 JAERI-M 93-222 h»; TWcomm® 1 9 9 3 *F11H wt &m • m*m-ffl • ±m B * 1 T * 1 K 3i Japan Atomic Energy Research Institute '-'AER1-M 93-222 トリア管の試作試験 1993年 11月 中村武彦・橋本和一郎・上塚 寛 丙野泰治・鈴木信幸‘ 日本原子力研究所 Japan Atomic Energy Research Institute JAERI- r! --93-222 JP9401176
Transcript of JP9401176 '-'AER 1-M JAERI-M 93-222...JAERI-H—93-222 JP9401176 JAERI-M 93-222 h»; TWcomm® 1 9 9...
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JAERI-H—93-222
JP9401176
J A E R I - M 93-222
h»; TWcomm®
1 9 9 3 *F11H
wt &m • m*m-ffl • ±m
B * 1 T * 1 K 3i Japan Atomic Energy Research Institute
'-'AER 1-M
93-222
トリア管の試作試験
1 993年 11月
中村武彦・橋本和一郎・上塚 寛
丙野泰治・鈴木信幸‘
日本原子力研究所
Japan Atomic Energy Research Institute
JAERI-r!--93-222
JP9401176
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JAHRI-M reports are issued irregularly. Inquiries about availability of the reports should be addressed to Information Division
Department of Technical Information, Japan Atomic Energy Research Institute, Tokai-mura. Naka-gun, Ibaraki-ken 319-11, Japan.
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Jよります
JAERI-M reports are issued irregularly
Inquiries about availability of the reports should be addressea to Information Division
Department of Technical Information， Japan Atomic Energy Research Institute， Tokai-
mura. Naka-別 n.1 baraki-ken 3 1 9・11.Japan.
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JAERI-M 93-222
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JAERI-M 93-222
Fabrication Test of Thoria Tube
Takehiko NAKAMURA, Kazuichiro HASHIMOTO, Hiroshi UETSUKA + *
Yasuharu NISHINO and Nobuyuki SUZUKI
Department of Reactor Safety Research Tokai Research Establishment
Japan Atomic Energy Research Institute Tokai-mura, Naka-gun, Ibaraki-ken
(Received October 1A, 1993)
An experimental research on fission product release from Light Water Reactor (LWR) fuels under accident conditions at high temperatures is planned and being prepared in Japan Atomic Energy Research Institute (JAERI), which is important for evaluating the impacts of the design base events and the severe accidents of the LWRs. Short segments of irradiated LWR fuels will be induction-heated in the tests. The release behavior of the fission products is going to be studied as a function of temperature under various atmospheres. Very stable material is required for the induction furnance which stands for high temperatures exceeding 2800°C under oxidizing or reducing atmospheres. Thorium dioxide (Thoria) which has a very high melting point of 3370°C and chemically stable at high temperatures is a strong candidate. However, because thorium is controlled by the government as nuclear fuel material, experiences of fabricating thoria components are very limited except for the uses as the nuclear fuels. Fabrication tests of thoria tubes from thoria powder were conducted to clarify the fabrication parameters. A thoria tube of outer diameter of about 35mm, inner diameter of about 24mm, length of about 145mm at density of about 90% to the theoretical, was successfully fabricated from the powder by rubber pressing and sintering.
Keywords: Thorium Dioxide (Thoria), Rubber Press, Fission Product ReJsase, Thoria Tube
+ Department of Hot Laboratories * Nuclear Fuel Industries
ii
JAERI-M 93-222
Fabrication Test of Thoria Tube
Takehiko NAKAMURA， Kazuichiro HASHIMOTO， Hiroshi UETSUKA + * Yasuharu NISHINO' and Nobuyuki SUZUKI
Department of Reactor Safety Research
Tokai Research Establishment
Japan Atomic Energy Research Institute
Tokai-mura， Naka-gun， Ibaraki-ken
(Received October 14， 1993)
An experimental research on fission product release from Light Water
Reactor (LWR) fuels under accident conditions at high temperatures is
planned and being prepared in Japan Atomic Energy Research Institute
(JAERI)， which is important for evaluating the impacts of the design base
events and the severe accidents of the LWRs. Short segments of irradiated
LWR fuels will be induction-heated in the tests. The release behavior of
the fission products is going to be studied as a function of temperature
under various atmospheres. Very stable material is required for the in-
duction furnance which stands for high temperatures exceeding 28000C under
oxidizing or reducing atmospheres.τhorium dioxide (Thoria) which has a
very high melting point of 33700C and chemically stable at high tempera-
tures is a strong candidate. However， because thorium is controlled by
the government as nuclear fuel material， experiences of fabricating thoria
components are very limited except for the uses as the nuclear fuels.
Fabrication tests of thoria tubes from thoria powder were conducted to
clarify the fabrication parameters. A thoria tube of outer diameter of
about 3Smm， inner diameter of about 24mm， length of about 14Smm at density
of about 90% to the theoretical， was successfully fabricated from the
powder by rubber pressing and sintering・
Keywords: Thorium Dioxide (Thoria)， Rubber Press， Fission Product
ReJ~ase ， Thoria Tube
+ Department of Hot Laboratories
* Nuclear Fuel Industries 11
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JAERI-M 93-222
@ &
1. 12 D tf> ( : 1 2. h y r © t t i 2
2. 1 #Jtt 2 2. 2 «C*ttg 3
3. h M T i W p 3 3. i &mmm 4
4. is & 9 5. £ t J6 9 m » 10 # # X IK 11 ttHI ORIGEN-2 (cJ; 5 HJ 7©JKS*l®§i tK©ft»§3l 39
Contents
1. Introduction 1 2. Properties of Thorium Dioxide (Thoria) 2 2.1 Material Properties 2 2.2 Radio Activity 3
3. Fabrication of Thoria Tube 3 3.1 Pellet Fabiration 4 3.2 Tube Fabrication by Rubber Pressing 6
4. Test 9 5. Summary 9 Acknowledgements 10 References 11
Appendix I Radio Activities of Thoria estimated with ORIGEN-2 Code , 39
iii
]AERI-M 93-222
目次
1.はじめに
2. トリアの性質・ H ・H ・....・ H ・H ・H ・...・ H ・.....・ H ・.....・H ・..........・ H ・...・ H ・.....・H ・..…… H ・H ・ 2
2. I 物性 ...・ H ・.....・ H ・...・H ・.....・ H ・...・H ・....・H ・-….....・H ・....・ H ・....・M ・-…...・ H ・......・H ・ 2
2. 2 放射能 ....・ H ・....・H ・....・ H ・...・ H ・-…・....・M ・-…....・ H ・.......・ H ・.....・H ・-…...・H ・ 3
3. トリア管試作 ....・H ・.......・ H ・........・H ・-…....・ H ・-…...・H ・...・ H ・..…...・H ・....・ H ・...・ H ・-… 3
3. 1 金型成型 ・…...・ H ・.........・ H ・....・ H ・-…・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・ 4
3.2 ラパープレス成型 H ・H ・.....・H ・...・ H ・..…....・H ・......・H ・.....・H ・-….....・H ・...・H ・ 6
4. 試験日 H ・H ・-…....・H ・-…...・ H ・-…・ H ・H ・..…...・ H ・............・ H ・.....・H ・....・H ・-…… 9
5. まとめ…・ H ・H ・..…...・ H ・..…H ・H ・...・ H ・..…H ・H ・......・ H ・.....・ H ・....・H ・...・ H ・.....・ H ・. 9
謝 辞 .....・H ・..…・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・ 10
参 考 文 献 …・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・・ 11
付録 I ORIGEN-2によるトリアの放射線強度の計算結果 ・H ・H ・..…...・ H ・....・ H ・...…・…. 39
Contents
1. Introduction
2. Properties of Thorium Dioxide (Thoria) •••••••••••••••••.•••••• 2
2.1 Material Properties • ••• •• • •••• •• ••••••• . •••••• ••••••• • •• ••• 2
2.2 Radio Activity ............................................. 3
3. Fabrication of Thoria Tube •••••••••••••••••••••••••••••••••••• 3
3.1 Pellet Fabiration ••• • ••••• • •• ••• • ••••••• • •••••• • ••••••• • ••• 4
3.2 Tube Fabrication by Rubber Pressing •••••.•••••••••••••••••• 6
4. Test •••••••••••••••••••••••••••••••••••••••••••••••.•••••••••• 9
S. Summary • • • • . • • • • • • • • • • • • • • • • • • • • • • • • • • • • • • • • • • • • • • • • • • • • • • • • • • 9
Acknowledgements •• ••• • • ••••• • ••••• . . ••• ••• . •••• •• • • •• •••• . . ••••• • • 10
References •••••••••••..••••••••••••••••••••••••••••••••••••••••••• 11
Appendix 1 Radio Activities of Thoria estimated with
ORIGEN-2 Code • • • • • • • • • • • . • • • • • • • • • • • • • • • . • • • • • . . • • • • • • 39
i
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JAERI-M 93-222
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]AER[-M 93-222
トリアは高温においても水蒸気との反応性は小さく[旬、金属ともほとんど反応しない。ニオ
ブ、タンタル、タングステンについては 1540 oC (1，813K)で1，OOOh以上接触をしていても
反応しない事が知られている[9]0
2. 2 放射能
天然にあるトリウムは、そのほぼ100%が232T hである。 232T hはα崩壊核種で、その
半減期は1. 41xI010年と非常に長くこの核種自身の比放射能は大きくない。しかし、
23 2T h はFig.5[lO]に示すトリウム系列 C4 n系列)で崩壊する。この系列に含まれる娘核種
は半減期数日以下の短半減期の核種が多いが、 22B R a および~2 B T hがそれぞれ半減期5.
76年および1. 91年と長く、これらが蓄積して行くことによって放射能が上昇して行く。
ORIGEN-2コードによる計算の結果、 100 gのトリウムを含む酸化トリウムは精製直
後、つまり 100%232Thの場合、その放射能は約 11μCi (4. lx105Bq)に過ぎ
ないが、 Fig.41こ示すように時間と共に上昇し、 50年後に約 10倍になりほぼ飽和する。崩壊
に伴って発生する中性子は毎秒1個程度と極わずかであり無視できるが、 7線については高エ
ネルギの7線を放出する20B T I等の娘核種が増えることから、放射能増加率を上回る増加率で7線の強度が上昇し、 50年後には初期強度の約2000倍に達する CFig.6)。発生する 7線
のエネルギ分布は、 Fig.71こ示す様に精製後短時間には娘核種の発生により大きく変化するが、
3カ月以降はさらに時間が経過しても大きくは変化しない。 ORIGEN-2コード[10]による
トリウム 100gの放射能および放出放射線の時間変化の計算結果を付録Iに示す。
照射済み燃料からのFP放出挙動を調べる実験では、 lOOOg程度のTh02を使用する計
画であり、精製後 10年以上を経過したトリウムを使用する可能性も高い。従って、ホットセ
ル外での取扱に於いては7線による被曝を小さくするための措置が必要となる。
3. トリア管試作
トリア管を試作するに先立って、金型成形により直径約 lOmm高さ約 lOmmのぺレットを
製作し、成形性、焼結性を調べた。ここでは、トリアの粉末処理、成形圧、焼結温度、焼結雰
囲気をパラメータとした。この結果を踏まえて、ラパープレス成形による管の試作を行った。
ここでは、粉末処理(パインダー効果を含む)、ゴム型形状、成形圧、焼結条件をノマラメータ
に成形性、焼結性を調べた。
試作に用いたトリア原料は、伝熱流動研究室が絶縁断熱材料として原研・東海研の核燃料倉
庫に保管していたトリア粉末約4. 9kgを使用した。試作作業のうち、粉末の調整、金型プレ
ス、焼結、試験検査は原子燃料工業・東海製造所で、ラパープレスは原研東海の融体・燃料プ
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JAERI-M 93-222
得られた造粒粉を使用することによって、充興密度は 2. 7 g/cm3程度が得られ、成型圧
11/cm2で-プレスすることにより十分な強度を存する加圧成型体が得られることが分かつた。こ
のl時、軸方向に加圧する構造のゴム型では、減圧時に軸方向に成型体を引きちぎろうとする力
が働くため、加圧は半径方向のみとするほうが良かった。焼結条件は、ペレットと同じ窒素雰
囲気で 16000Cで十分な焼結結果が得られた。粉末にパインダーとしてPVAを添加した試
作では、加圧成型までは問題がなかったが、;焼結はうまく進まない結果となった。
謝 辞
本研究を行うに当たっては、伝熱流動研究室の村尾良夫室長のご厚意により卜リア粉末を提
供して頂きました。また、ラパープレスの使用に当たっては、融体・燃料プロセス研究室の高
橋良寿氏、山岸滋氏、ならびに小川徹室長の協力を得ました。記して感謝します。さらに、数
回に及ぶトリアの受払し、については、沼田和義氏をはじめとして核燃料課諸氏の協力を得まし
た。また、トリア粉末の調整、焼結等の作業においては高野文夫氏をはじめとする原子燃料工
業・新型炉燃料部の諸氏の協力を得ました。ここに、記して感謝します。
一lOー
-
JAERI-M 93-222
# # x m [1] M. Kanno, "Physical and Chemical Properties of Thorium Fuel".
[2] Ohnysty and Rose, J. Am. Chem. Soc. 47, p. 398, 1964.
[3] WAPD-TM-618 Add. I, p. l l , (402).
[4]m7kFmm&z>£^m$mm.&, * WKpmm^^t^", *ar+xh->'j-XNo.3, NEN-ANSEN No.13, MH&A K-?7J$£#F35f£^ 1985.
[5] D. L. Hagrman et al., "MATPRO Version 11 (Revision 2), A Hand Book of Material
Properties for Use in the Analysis of Light Water Reactor Fuel Rod Behavior",
NUREG/CR-0479, TREE-1280, Rev.2 R3 and R4, EG&G Idaho, 1981.
[6] T. Tachibana, et al., "Dependence on Strain Rate and Temperature Shown by Yield
Stress of Uranium Dioxide", J. Nucl. Sci. Technol. 13[9], pp. 497~502, 1976.
[7] R. Benz, "Thorium-Thorium Dioxide Phase Equilibria", J. Nucl. Mater. 29, 43, 1969.
[8] J. M. Markowitz and J. C. Clayton, "Corrosion of Oxide Nuclear Fuels in High Temperature Water", Bettis Atomic Power Lab. WAPD-TM-909, 1970.
[9] S. Peterson and C. E. Curtis, "Thorium Ceramic Data Manual", Vol. I, p. 22, ORNL-4503, 1970.
[io] ttmim ti!k • mm-5?~j r , */ ,«& 19 8 2.
[11] A. G. Croff, et al., "Revised Uranium-Plutonium Cycle PWR and BWR Models for
the ORIGEN Computer Code", ORN1/TM-6051, 1978.
- 11 --
]AERI-M 93-222
参考文献
[1] M. Kanno， "Physi回 1and Chemical Properties of Thorium Fuel".
[2] Ohnysty and Rose， J. Am. Chem. Soc. 47， p. 398， 1964.
[3] WAPD-TM-618 Add. 1， p.ll， (402).
[4]軽水炉燃料のふるまい編集委員会、"軽水炉燃料のふるまい"、実務テキストシリーズNo.3，
NEN-ANSEN No.13，財団法人原子力安全研究協会、 1985.
[5] D. L. Hagrrnan et al.， "MATPRO Version 11 (Revision勾， A Hand Book of Material
Properties for Use in批Analysis of Light Water Reactor Fuel Rod Behavior"，
NUREG/CR-0479， TREE-1280， Rev.2 R3 and R4， EG&G Idaho， 1981.
[6] T. Tachibana， et al.， "Dependence on Strain Rate and Temperature Shown by Yield
Stress of Uranium Dioxide九J.Nucl. Sci. Technol. 13[9]， pp. 497-502， 1976.
[7] R. Benz， "Thorium-Thorium Dioxide Phase Equilib巾ヘ1.Nucl. Matcr.空， 43，1969.
[8] J. M. Markowitz印 dJ. C. Clayton， "Corrosion of Oxidc Nuclear Fuels in High
Temperature Water"， Bettis Atomic Powcr Lab. WAPD-TM-909， 1970.
[9] S. Pctcrson and C. E. Curtis， "Thorium Ccramic Data Manual"， Vol. 1， p. 22， ORNL-
4503， 1970.
[10]村上悠紀雄他、"放射線データブック"、地人書館、 1982.
[11] A. G. Croff， et al.， "Revised Uranium-Plutonium Cycle PWR and BWR Modc1s for
出eORIGEN Computer白 de"，ORNl/fM-6051， 1978.
-噌
A
-
JAKRI-M 93-222
Table 1 Physical properties of thorium compoundsdJ
Metal Oxide Carbide
Chemical Form
Th Th0 2 ThC ThC2
Crystal Structure
FCC (1360°C)
FCC CaF2 type
FCC NaCl type
a Monoclinic 0 Tetragonal
r FCC
Density, g/cm3 11.72 (25° C) 10.00 (27° C) 10.63 a 9.6 0 8.76 r 8.68
Melting Point, 'C
1750 3370 2500 a 1440 /8 1490 r 2610
Thermal Conductivity,
W/cm K
0.140 (27° C)
Elastic
Modulus, MPa
7.24x10" 2x10 s - -
12
J^E1{I~ M 93-222
Table 1 Physical properties of thoriurn cornpounds[l]
時letal Oxide Carbide
Chemical Th ThOz ThC ThCz
Form
Crystal FCC ( 13600
c) CaF2 type NaCl typ巴 βTetragonal
r FCC
Density， g/cmJ 11. 72 (25-c) 10.00 (27-c) 10.63 α9.6 β8.76
r 8.68
Melting Point， 1750 3370 2500 α1440 'C s 1490
r 2610
Thermal 0.140 (270
c)
Conductivity，
W/cm K
EJastic 7.24x104 2x105
I Modulus， MPa
12
-
JAERI-M 93-222
Table 2 P r o p e r t i e s of Th0 2 and U0 2
T h 0 2 I W ) - " U0 2 4 l i 5 W >
Crystal Structure
Lattice Constant, A
FCC
CaF 2 type
5.5971 (300K)
FCC
CaF 2 type
5.469
Density, g/cm 3 10.001 (300K) 10.96
Melting Point, *C 3,300~3,370 2,805~2,865
Thermal Conductivity,
W/m K
14.0 (300K)
4.0 (l,0OOK)
8.0 (300K)
3.5 (l.OOOK)
2.2 (2.000K)
Specific Heat,
J/kg K
225 (300K)
290 (l.OOOK)
325 (1.800K)
230 (300K)
310 (l.OOOK)
375 (2.000K)
Coefficient of Thermal
Expansion, 1/K
8xl0" 6 (300K)
1x10"' (l.OOOK)
1.2x10-' (2,000K)
8 ~ 6 x l 0 " 6 (300K)
1.1x10"' (l.OOOK)
1.6x10"' (2.000K)
Vapor Pressure, Pa
~ 0 . 3 (2,600K)
~ 0 . 1 (2.000K)
20 (2.600K)
1000 (3.000K)
Tensile Strength, MPa l x l O 2 (300K) 3 x l 0 2 (1.200K)
l x l O 2 (2.000K)
Elastic Modulus, MPa 2x10 s (300K) 2 .1xl0 5 (300K)
1.9x10' (l.OOOK)
1.2x10' (2.000K)
- 1 3 -
]AERI-M 93-222
Table 2 Properties of Th02 and U02
ThOZ1)，2)，Jl UO
Z4l.Sl.の
Crystal Structure FCC FCC
Lattice Constant， A CaF2 type CaF2 type
5.5971 (300K) 5.469
Density， g/cmJ 10.001 (300K) 10.96
品feltingPoinら.C 3，300-3，370 2，805-2，865
Thermal Conductivity， 14.0 (300K) 8.0 (300K)
W/m K 4.0 (1，000K) 3.5 (1，000K)
2.2 (2，000K)
Specific Heat， 225 (3ooK) 230 (300K)
J!kg K 290 (I，OOOK) 310 (I，OOOK)
325 (1，800K) 375 (2，000悶
Coefficient of Thermal 8xlO-6 (300K) 8-6xlO-6 (300K)
Expansion， llK lxlO-5 (I，OOOK) 1.lxlO-5 (I，OOOK)
1.2xlO-5 (2，000K) 1.6xlO-5 (2，000K)
Vapor Pressure， Pa -0.1 (2，000K)
-0.3 (2，600K) 20 (2，600K)
1000 (3，000K)
Tensile Strength， MPa lxl02 (300K) 3x102 (1，200K)
1x102 (2，0∞K) Elastic Modulus， MPa 2xlOS (300K) 2.1x105 (300K)
1.9x105 (l，OOOK)
1.2x105 (2，000K)
。δ咽
i
-
JAERl-M 93-222
Table 3 Bulk d e n s i t y of o r i g i n a l Th0 2 powder
Rot No. Density, g/cm3
1 0.87
2 0.83
3 0.94 J
4 0.91 1
Table 4 Summary of ThC>2 p e l l e t f a b r i c a t i o n t e s t c o n d i t i o n s
Powder Milling Time, h
Pressing Pressure,
t/cm3
Sintering Conditions
Original - 2 1500° C, for 2h, in Air, (320° C/h)
Ball Milled 2 3 1300° C, for 2h, in N2, (320° C/h)
Ball Milled
24 4 1600° C, for 2h,
in N2, (320° C/h)
- 14 -
JAERI-M 93-222
Table 3 Bulk density of original Th02 pm.Jder
Rot No. Density，
glcm3
1 0.87
2 0.83
3 0.94
4 Q.91
Table 4 Summary of Th02 pellet fabrication test conditions
Powder MilIing Pressing Sintering Conditions
Time， h Pressure，
t/cm3
Original 2 1500. C， for 2h，
泊 A討， (320.C/h)
Ball MiIled 2 3 1300. C， for 2h，
in N2， (320・C/h)
24 4 1600・C，for 2h，
in N2， (320. C/h)
ー 14
-
JAERI-M 93-222
Table 5 Green and sintered densit ies obtained in pel le t fabrication t e s t s
Powder Sintering Condition
Green Density Powder Sintering Condition Sintered Density, g/cm3
Powder Sintering Condition
Pressing Pressure
Powder Sintering Condition
2 l/cm2 i t/cm2 4 t/cm2
Original 1500* C, Air 4.54 8.18
4.92 8.67
5.07 8.84
Original
1300* C, N 2 4.54 7.88
4.92 8.69
5.07 8.74
Original
1600' C, N 2 4.54 8.63
4.92 9.29
5.07 9.11
Milled 2h
1500' C, Air 4.53 8.91
4.86 8.58 8.83
Milled 2h
1300* C, N 2
Milled 2h
1600'C, N 2 4.53 8.93
4.88
9.11 4.95
9.29
Milled 24h
1500* C, Air Milled 24h
1300* C, N 2
Milled 24h
1600'C, N 2 4.66 9.29
4.89 9.18
5.08 9.20
- 15 -
]AER1-M 93-222
Table 5 Green and sintered densities obtained in pellet fabrication tests
Powder Sintering Green Density
Condition Sintered Density， glcm3
Pressing Pressure
2 t/cm2 3 t/cm2 4 t/cm2
Original 1500・C，Air 4.54 4.92 5.07 8.18 8.67 8.84
1300・C，N2 4.54 4.92 5.07 7.88 8.69 8.74
1600・C，N2 4.54 4.92 5.07 8.63 9.29 9.11
Milled 1500・C，Air 4.53 4.86 4.98 2h 8.91 8.58 8.83
1300・C，N2 一 一
1600・C，N2 4.53 4.88 4.95 8.93 9.11 9.29
Milled 1500・C，Air 一 一24h
1300・C，N2 一
1600・C，N2 4.66 4.89 5.08 9.29 9.18 9.20
phd
唱
i
-
JAERI-M 93-222
Table 6 Rubber p ress t e s t parameters
Rubber
Type I n I IV
Rubber
Outer Dia., mm 50 (30) 50 (30) 50 (30) 50 (30)
Rubber Inner Dia., mm 30 (24) 10(8) 30 (24) 30 (24)
Rubber Length, mm 190
(150) 190
(150)
300 (240)
190
(150)
Rubber
Axial Pressing Stroke, mm
5 5 5 0
Powder A1 20 3 Powder
Th0 2 original Th0 2 milled, 2h
Th0 2 granulated Th0 2 granulated with PVA
Pressing Pressure, t/cm2 0.3 0.4 1.0 2.0
| Separator Zinc stearate coated stem Teflon coated stem
Pressing Direction Radial & Axial (Rubber type I , I I , I ) Radial (Rubber type IV) |
Dimensions of the rubber molds under atmospheric pressure are listed. Figures in ( ) are those expected after sintering.
- 1 6 -
]AERI-M 93-222
Table 6 Rubber press test parameters
Type E E W
Outer Dia.， mm 50 (30) 50 (30) 50 (30) 50 (30)
Inner Dia.， mm 30 (24) 10 (8) 30 (24) 30 (24) Rubber
Length， mm 190 190 300 190
(150) (150) (240) (150)
Axial Pressing 5 5 5 。Stroke， mm
Powder Al203
百102original
Th02 milled， 2h
百102granulated
百102granulated with PV A
Pressing Pressure， t/cm2 0.3
0.4
1.0
2.0
Separator Zinc stearate coated stem
Teflon coated stem
Pressing Direction Radial & Axial (Rubber type 1， n ， m) Radial (Rubber type N)
Dimensions of the rubber molds under atrnospheric p民ssureare listed.
Figures in ( ) are those expected after sintering.
→ 16
-
JAERI-M 93-222
Table 7 Summary of rubber p r e s s t e s t cond i t i ons
Test No.
Rubber Type
Powder Type
Thoria Mass, g
Separator Pressing Condition
Sintering Condition
1 I Original 348 no 1 t/cm2, 5m -
2 I Original 348 no 2 t/cm2, 5m -
3 I Original 486 no 2 t/cm2, 5m -
4 I Original 312 Zinc Stearate
0.3 t/cm2, 5m
5 I Original 301 Zinc Stearate
0.4 t/cm2, 5m -
6 n Original 500 Teflon 1 l/cm2, 5m -7 n Milled, 2h 700 Teflon 0.4 t/cm2, 5m 1600° C,
2h in N 2 (100° C/h)
8 n Granulated 990 Teflon 0.3 t/cm2, 5m 1 t/cm2, 30m
9 IV Granulated 624.3 Teflon ditto 1600° C, 2h in N 2 (50° C/h)
10 IV Granulated with PVA
Teflon ditto 1600° C, 2h in N 2 (100° C/h)
- 17 -
]AER[-M 93-222
Table 7 Summary of rubber press test conditions
Test Rubber Powder Thoria Separator Pressing Sintering
No. Type Type Mass， g Condition Condition
1 Original 348 no 1ν'cm2，5m
2 Original 348 no 2ν'cm2，5m
3 E Original 486 no 2ν'cm2，5m
4 Original 312 Zinc 0.3ν'cm2，5m
Stearate
5 I Original 301 Zinc 0.4 t/cm2， 5m
Stearate
6 E Original 500 Teflon 1 t/cm2， 5m
7 E Milled， 2h 700 Teflon 0.4 t/cm2， 5m 1600.C，
2h in N2
(100-C!h)
8 E Granulated 990 Teflon 0.3 t/cm2， 5m
1 t/cm2， 30m
9 W Granulated 624.3 Teflon ditto 1600. C，
2h in N2
(50-C!h)
10 W Granulated Teflon ditto 1600. C，
with PVA 2h in N2
(100-C!h)
一17ー
-
JAEKI-M 93-222
Table 8 Summary of rubber press tes t resul ts
Test No.
Test Conditions Filled Density, g/cm3
As Pressed As Sintered Rubber Type
1 Original Powder 1 t/cm2
1.5 4.3 g/cm3, 4mm thick (Photo. 9)
- I
2 Original Powder 2 t/cm2
1.5 (Photo. 9) - I
3 Original Powder 2 t/cm2, 3001
1.3 5.2 g/cm3, 3mm thick (Photo. 9)
- III
4 Zinc stearate 0.3 t/cm2
1.3 4.1 g/cm3, 4mm thick
(Photo. 10, 11)
Cracked II
5 Zinc stearate 0.4 t/cm2
1.3 (Photo. 10) - II
6 Inner Dia. 10mm Teflon
1.4 2 axial cracks (Photo. 12)
- II
7 Milled Powder I.D. 10mm
Teflon
2.0 4.3 g/cm3 O.D. 34.5mm
I.D. 10mm Length 144mm
Round Crack
7.0 g/cm3 O.D. 29.5mm
I.D. 8mm Length 120mm
(Photo. 13)
I
8 Granulated I.D. 10mm
2.8 4.8 g/cm3 O.D 39.1mm I.D. 10mm
Length 144mm Round Crack (Photo. 14)
I
9 Granulated No Axial Press
2.7 624.3 g 4.6 g/cm3
O.D. 42.9mm I.D. 30mm
Length 182.3mm
609.9 g 8.2 g/cm3
O.D. 35.2mm I.D. 24.2mm
Length 145.1mm (Photo. 15)
IV
10 Granulated with PVA
No Axial Press
2.7 - (Photo. 15) IV
18 -
JAE]{[-M 93-222
Table 8 Summary of rubber press test results
Test Test Conditions Filled As Pressed As Sintered Rubber No. D6encsmitそy， Type
1 Original Powder 1.5 4.3 glcm3， 1νcm2 4mm thick
(Photo. 9)
ウ“ Original Powder 1.5 (Photo. 9) I 2 t/cm2
3 Origt/incaml 2 Powder 1.3 5.2 glcm3， III
2 t/cm"， 3001 3mm thick (Photo. 9)
4 Zinc stearate 1.3 4.1 glcm3， Cracked II 0.3 t/cm2 4mm thick
(Photo. 10， 11)
5 Zinc stearate 1.3 (Photo. 10) II 0.4 t/cm2
6 Inner Dia. lOmm 1.4 2 axial cracks 11 Teflon (Photo. 12)
7 Milled Powder 2.0 4.3 glcm3 7.0 glcm3
I.D. lOmm 0.D.34.5mm 0.D.29.5mm Teflon I.D. 10mm I.D.8mm
Length 144mm I£(PElhuolt1o
120mm Round Crack . 13)
8 Granulated 2.8 4.8 glcm3 I
I.D. lOmm O.D 39.1mm I.D.lOmm
Length 144mm Round Crack
σhoto. 14)
9 Granulated 2.7 46.62463cmg 3 6096.9cmg 3
IV
No Axial Press 8.2 O.D.42.9mm 0.D.35.2mm I.D. 30mm I.D.24.2mm
Length 182.3mm kT(IPEdh1oto14.51.51m) m
10 Granulated 2.7 ー (Photo. 15) IV with PVA
No Axial Press
18 -
-
JAERI-M 93-222
Table 9 Dimensional measurement r e s u l t s of TI1O2 tube f a b r i c a t e d i n t e s t No.9
Dimension, mm Weight,
g Density, g/cm3 Outer
Diameter top x, y
middle x, y bottom x, y
Inner Diameter top x, y
bottom x, y
Length
max.
mill.
Weight, g
Density, g/cm3
As Pressed
45.0, 44.0 30.0, 30.0 185.0
624.3 4.6 As
Pressed 42.7, 41.9 ~ y ""
624.3 4.6 As
Pressed 41.8, 42.1 30.0, 30.0 179.5 624.3 4.6 As
Pressed
ave. 42.9 ave. 30.0 ave. 182.3
624.3 4.6
As Sintered
35.8, 36.0 24.1, 24.2 147.1
609.9 (98%)
8.2 As
Sintered 33.8, 34.0 _ ^ —
609.9 (98%)
8.2 As
Sintered 37.3, 34.0 24.0, 24.3 143.1 609.9 (98%) 8.2
As Sintered
ave. 35.2 (82%)'
ave. 24.2 (81%)'
ave. 145.1 (80%)'
609.9 (98%)
8.2
' (As sintered)/(As pressed)* 100
- 19 -
As Pressed
As Sintered
]AERI-M 93-222
Table 9 Dimensional measurement results of Th02 tube fabricated in test No.9
Dimension， mm
Outer Weight，
Inner Length g Diameter Diameter top x， y top x， y ma"'i.
middle x， y bottom x， y bottom x， y mm.
45.0， 44.0 30.0， 30.0 185.0
42.7， 41.9 ，
41.8， 42.1 30.0， 30.0 179.5 624.3
ave. 42.9 ave. 30.0 ave. 182.3
35.8， 36.0 24.1， 24.2 147.1
33.8， 34.0 ， ー
37.3， 34.0 24.0， 24.3 143.1 609.9 (98%)
ave. 35.2 ave. 24.2 ave. 145.1 (82%)' (81%)" (80%)"
• (As sintered)/(As pressed)*100
- 19
Density， glcmJ
4.6
8.2
-
JAERI-M 93-222
Fission Product Release Test Facility
STEAM/GAS SUPPLY SYSTEM
OPTICAL PYROMETER
Fig. 1 Schematic of fission product release test facility
20
JAER[~M 93~222
Fission Product Release Test Facility
ii伯釘JT:回世F-::::;::
STEAM/GAS SUPPLY SYSTEM
OPTICAL PYROMETER
Fig. 1 Schematic of fission product release test facility
一 20ー
-
JAERI-M 93-222
Cooling Water pzq
— He
Zirconia (Thoria) Quartz Tube
.Induction Coil
fqSf^Test Fuel
Carbon Suseptor
Zirconia Insulator
Cooling Water
(Unit: mm)
Fig. 2 Schematic of induction heater for the fission product release test
- 21 -
He
JAERI-M 93-222
Zirconia
→ He
Zirconia (Thorial
Quartz Tube
Induction Coi I
Fuel
Suseptor
Zirconio Insulator
( Unit : mm )
Fig. 2 Schematic of induction heater for the fission product release test
-21
-
JAERI-M 93-222
Fig. 3 The Th-Th02 phase diagram^7]
1 i i l 1 V I 1 1 1
Th02 \
Th0 2-!%\ \ -
U02
\
Th02-5% \ \ U0 2 x \ \
ThOz-IO0^
-
JAERI-M 93-222
Th
90
"2Th,Th
1.41X10l0y
22STh,RdTh
/ 1.913y
Ac
89
a (y)
228Ac,MsTh2
/ 6.13h (?) a,7
Ra
88
2 2 8Ra, MsTh!
5.76y
4 »Ra,ThX 3.66d
F r
87 air)
Rn
86
220Rn,Tn
55.6s
At
85 «O0
Po
84
216Po,ThA
0.15s
2 1 2Po,ThC
^3.05X10~7s
Bi
83 a
212Bi,ThC
/ 60.60m
$(64.0%) 7 1"
Pb
82
212Pb,ThB
10.64h
/ (36.0%)
^Pb.ThD
Tl
81
2 0 8Tl,ThC
3.053m
7
Fig. 5 Decay chain of 232Th[10]
- 23 -
JAERI-M 93-222
Th 2~2Th，Th ~2S Th，RdTh
90 1.41 X 1010y 〆1.913y
Ac 228Ac，MsTh2
89 〆6.13hRa 228Ra， MsTh1 ~ 224Ra，ThX
88 5.76y 3.66d
Fr
87
Rn 220Rn，Tn
86 55.6s
At
85
PO 216PO，ThA 212PO，ThC'
84 0.15s ~3.05X 1O-7s
Bi 212Bi，ThC
付d 83 〆60.60mPb 212Pb，ThB Y
|み却8Pb，ThD
J
82 10.64h ， 安定Tl EωTl，ThC' /β 川Y 81 3.侃3m
Fig. 5 Decay chain of 232Th[lO]
23
-
JAERI-M 93-222
10000 HIST/TH02
o _• ! 000
LJ
< I
00
X-ray Intensity
" ^ O M ' O M e V / s R a d i o A c r i v i t y 1UCi(4.lxl0 5Bq)
— at t = Q 0.
T IME (y ) 100
Fig . 6 Gamma-ray intensity and ratio activity of thorium dioxide (Thoria) as a function of time
SPECTRUM/ TH02
0.1 I
X-RAY ENERGY (MeV) 10
Fig. 7 History of -y-ray spectrum emitted from thorium dioxide (Thoria)
- 24 -
JAERI-M 93-222
HIST/TH02
r -ro y 1 n↑ensi↑y ---------
10ド二:ぢ5x102MeV/5ot t = 0 11μCiJ4.lxIO
V
Bq) 干 ott=
ハUハυハUハU(()"↑↑o-0.一)〉ト目的
Z凶↑
ZH
1000
100
凶〉一↑4」凶匡 100 10 0.1
( y )
Gamma-ray intensity and ratio activity of thorium dioxide (Thoria) as a function of time
TIME
Fig. 6
SPECTRUM I TH02 10
6
105
_ 104 vl ¥10-g 102 4炉・・~ 10 ιl )1O l
ト 16~~ 10" z 10可巳10-5z 10-. ~ 167
168
0.01 10 0.1
(MeV)
History of y目 rayspectrum emitted from thorium dioxide (Thoria)
24ー
ENERGY r -RAY
Fig. 7
-
Th0 2 ORIGINAL POWDER
2 3 4 PRESSURE ( t / c m 2 )
Fig. 8 Pressing pressure and green density of Th0 2 pellets made of original powder
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Fig. II
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JAERI-M 93-222
Silicone Rubber Upper Plug (No.50)
Thoria Tube
Stainless Steel Core (Type 304)
Silicone Rubber Tube (No.50)
Silicone Rubber Lower Plug (No.50)
Fig. 13 Design of silicone rubber molds
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Photo. 1 Appearance of the original thoria powder.
Photo. 2 Compressor and mold for pellet fabrication tests.
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Photo. 1 Appearance of the original thoria powder.
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Photo. 2 Compressor and mold for pellet fabrication tests.
29
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JAICRI M 9:i 222
Photo. 3 Mold for pellet fabrication tests.
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30
J\"I~I ~1 9:1 222
Photo. 3 Mold for pellet fabrication tests.
Photo. 4 Milling machine for thoria powder.
30
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JAKKI M 9.1 222
Photo. 5 Thoria pellets as pressed.
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JAICR1 M 93-222
Photo. 9 Appearance of pressed thoria tubes in fabrication tests No.l (left), No.2 (right) and No.3 (center). The rubber mold type HI is seen behind them.
Photo, 10 Appearance of pressed thoria tubes in fabrication tests No.4 (left) and No.5 (right).
34
J八Iml M 93-222
Photo. 9 Appearance of pressed thoria tubes in fabrication tests No.1 (left)， No.2 (right) and No.3 (center). The rubber mold type DI is seen behind tnem.
Photo， 10 Appearance of pressed thoria tubes in fabrication tests No.4 (left) and No.5 (right).
34ー
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JAKRI M 9.1 222
Photo. 11 Pressed thoria tube disassembled from the core in fabrication test No.4. The tube was cracked into 4 pieces during the disassembling. The rubber molds type I are seen behind.
Photo. 12 Appearance of pressed thoria tube in fabrication test No.6.
35
j八EI{I ~1 9:1 222
Photo. 11 Pressed thoria tube disassembled from the core in fabrication test No.4. The tube was cracked into 4 pieces during the disassembling・ Therubbcr molds type 1 are seen behind.
Photo. 12 Appearance of pressed thoria tube in fabrication test No.6.
35
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JAKRI M 93 222
Photo. 13 Appearance of sintered thoria tube in fabrication test No.7. The longitudinal crack was generated during the sintering at 1600°C for 2h in N2 atmosphere, in addition to the radial cracks which were generated during the pressing stage.
Photo. 14 Appearance of pressed thoria tube in fabrication test No.8.
36
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JAKRI-M 93-222
Photo. 15 Appearance of sintered thoria tubes fabricated in tests No.9 (right) and No.10 (left).
37 -
jAERI-M 93-222
Photo. 15 Appearance of sintered thoria tubes fabricated in tests No.9 (right) and No.10 (left).
37
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JAICK! M 93 222
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JAERI-M 93-222
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39
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JAERI-M 93-222
J O G L O G S Y S T E M S Y S N 0 0 E S U N
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ACE TABLE OF CONTENTS ON UNIT - 12 FOR OUTPUT UNIT - 6 t ORIGEN2 OVERVIEW AND DOCUMENTATION 3 INPUT ECHO; READ ON 5 LIST ON 6 COPY TO 50 5 NEUTRON YIELD PER NEUTRON-INDUCED FISSION 6 (ALPHA,N) NEUTRON YIELD PER FISSION 7 SPONTANEOUS FISSION NEUTRON YIELD PER FISSN 8 INDIVIDUAL ELEMENT FRACTIONAL RECOVERIES
10 GROUP ELEHENTAL FRACTIONAL RECOVERIES 11 ELEMENTAL ASSIGNNHENT TOFRAC RECOVERY GROUP 12 ELEMENTAL CHEHICAL TOXICITIES
13 ORIGEN INSTRUCTIONS FDR THIS CASE
14 OUTPUT TABLES--TITLE= IRRADIATION OF NSRR FUEL AT A NATURAL PULSE 00004300 RECYCLE > = 0 14 REACTIVITY AND BURNUP DATA
"ACTIVATION PRODUCTS*****ACTIVATION PRODUCT5**«*«ACTIVATION PRODUCTS ACTIVATION P R O D U C T S " " *ACTIH10ES * DAUGHTER5***ACTINIDES t DAUGHTERS***ACTINIDES + OAUGHTERS***ACTINIDES * DAUGHTERS**
15 ALPHA RADIOACTIVITY FRACTIONAL CURIES SUHHARY TABLE: *FISSION PRODUCTS********FISSION P R O D U C I S * " " * " F I S S I O N PRODUCTS********FISSION PRODUCTS*******
16 (ALPHA,N) NEUTRON SOURCE 17 SPONTANEOUS FISSION NEUTRON SOURCE 18 ACTIVATION PRODUCT PHOTON TABLE (_ 1 20 ACTINIDE NUCLIDE PHOTON TABLE > 24 FISSION PRODUCT NUCLIDE PHOTON TABLE M
26 ORIGEN INSTRUCTIONS FOR THIS CASE I
27 OUTPUT TABLES--TITLE= COOLING TIHE STEP (NSRR FUEL ROD IRRADIATED IN THE NSRR 00014400 RECYCLE 1 = 0 cS 27 REACTIVITY AND BURNUP DATA |
"ACTIVATION PR0DUCTS*"**ACTIVAT10N PRODUCTS*****ACTIVATI0N PRODUCTS*****ACTIVATI0N PRODUCTS**** to *ACTINIDES * DAUGHTERS***ACTINIDES + DAUGHTERS***ACTINIDES + OAUGHTERS***ACTINIDES * DAUGHTERS** to
28 CONCENTRATIONS, GRAMS SUHMARY TABLE: 30 RADIOACTIVITY, CURIES SUHHARY TABLE:
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t t m i t » » » » u M Mixttitiiiiuitinxxiiiiuitmixtixiii 1 ttinx >************ 0RIGEN2: A REVISED AND UPDATED VERSION OF THE ORIGEN COMPUTER CODE ****•**»«» tttivxif"iiiiitiiitiitiiitiiii>i«>iiiiiji)tfiitxtimtiiiitiiit«titifiitxiiixi»tiii»itxii
INTRODUCTION THIS TEXT IS INTENDED TO BE A BRIEF OUTLINE OF THE 0RIGEN2 COMPUTER CODE, WHICH IS A REVISED AND UPDATED VERSION OF THE OHIGEN DOCUMENTED IN REPORT ORNL-4628 (MAY 1973). INCLUDED HERE ARE A BRIEF DESCRIPTION OF THE FUNCTIONS OF ORIGEN2, A LISTING OF THE MAJOR DATA SOURCES, A LISTING OF THE PUBLISHED DOCUMENTATION CONCERNING ORIGEN2, AND AN OUTLINE OF THE ORIGEN2 OUTPUT ORGANIZATION. ORIGEN2 IS AVAILABLE FROM THE ORNL RADIATION SHIELDING INFORMATION CENTER (RSIC) AT THE FOLLOWING AODRESS:
CODES COORDINATOR RADIATION SHIELDING INFORMATION CENTER BLDG. 6025 OAK RIDGE NATIONAL LABORATORY OAK RIDGE, TENNESSEE 37S30 PHONE: (615) 574-6176
QUESTIONS CONCERNING 0RIGEN2 SHOULO BE ADDRESSED TO RSIC. DESCRIPTION
0RIGEN2 IS A REVISION AND UPDATE OF THE ORIGEN COMPUTER CODE. SPECIFICALLY, THE INPUT, OUTPUT, CONTROL, AND DATA OF ORIGEN HAVE BEEN SIGNIFICANTLY REVISED AND UPDATED TO REFLECT CURRENT INFORMATION ANO NEEDS. IT SHOULO BE NO
HATHEHATICAL METHODS USED TO SOLVE THE NUCLIDE BUILDUP, DEPLETION, ANO DECAY EQUATIONS ARE ESSENTIALLY UNCHANGED ORIGEN. 0RIGEN2 IS A COMPUTER CODE DESIGNED TO CALCULATE THE COMPOSITION AND CHARACTERISTICS OF NUCLEAR MATERIAL FUNCTION OF DECAY TIME ANO THE CHANGES THE HATERIALS UNDERGO DURING VARIOUS FUEL CYCLE OPERATIONS. INPUT AND OUTI HAVE BEEN DESIGNED TO FACILITATE FLEXIBILITY IN THE TYPE OF CASES THAT CAN DE CONSIDERED AND IN CONTROLLING THE Dl OUTPUT. FOR FURTHER INFORMATION, THE USER IS REFERRED TO THE DOCUMENTATION LISTED BELOW.
MAJOR DATA SOURCES VIRTUALLY ALL ASPECTS OF THE DATA INPUT TO 0RIGEN2 HAVE BEEN UPDATED OR REVISED TO REFLECT CURRENT INFORMATION PRINCIPAL SOURCES OF CROSS SECTION DATA WERE THE ENDF/B-IV, ENDF/8-V, AND LENDL COMPILATIONS. DECAY ANO PHOTON I WERE PRIMARILY BASED ON THE EVALUATED NUCLEAR STRUCTURE DATA FILE (ENSDF) AT ORNL ANO ENDF/B-IV. DATA CONCERNING AND FUEL CHARACTERISTICS WERE OBTAINEO FROH REFERENCE SAFETY ANALYSIS REPORTS AND, WHERE POSSIBLE, THE COMMERCIAL VENDORS.
DOCUMENTATION THE FOLLOWING ITEHS CONSTITUTE THE 0R1GEN2 DOCUMENTATION PUBLISHED AS OF THE DATE OF THIS CODE PACKAGE:
A.G. CROFF, -0RIGEN2 - A REVISED AND UPDATED VERSION OF THE OAK RIDGE ISOTOPE GENERATION AND DEPLETION CODE", ORNL-5621 (JULY 19B0). A.G. CROFF, "A USER'S HANUAL FOR THE 0RIGEN2 COMPUTER CODE", OHNL/TH-7175 (JULY 1980). A.G. CROFF, H.A. BJERKE, G.W.MORRISON, ANO L.H. PETRIE, 'REVISED URANIUM-PLUTONIUM CYCLE PWR AND BWR MODELS FOR THE ORIGEN COMPUTER CODE", ORNL/TH-6051 (SEPTEMBER 1978). A.G. CROFF AND H.A. BJERKE, 'ALTERNATIVE FUEL CYCLE PWR MODELS FOR THE ORIGEN COHPUTEH CODE', ORNL/TM-7005 (FEB 1980). A.G. CROFF, R.L. HAESE, AMD H.B. GOVE, "UPDATED DECAY AND PHOTOH LIBRARIES FOR THE ORIGEN CODE', ORNL/TH-6055 (FEB 1979) A.G. CROFF, '0RIGEN2: A REVISED AND UPDATED VERSION OF ORIGEN', TRANS. AM. NUCL. S O C , VOL. 3A, P. 349-50 (JUNE 19S0).
BASE ASPECTS TED THAT THE FROH THAT IN S AS A PUT FEATURES ETAIL OF THE
THE NFORHATION REACTOR REACTOR
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